One-Pot Synthesis of Conductive Metal–Organic Framework@polypyrrole Hybrids with Enhanced Electromagnetic Wave Absorption Performance

Rational heterostructure design can bring interfacial polarization relaxation to significantly enhance the electromagnetic wave (EMW) absorption performance. However, intelligently building a homogeneous heterostructure with superior EMW absorption properties remains a great challenge. Herein, a typical conductive metal–organic framework Cu₃(HHTP)₂ (hexahydroxytriphenylene, HHTP) is delicately packed onto a polypyrrole (PPy) conductive polymer surface via a one-step in situ polymerization approach. Results show that Cu₃(HHTP)₂ is well packed on the PPy surface to form an elegant Cu₃(HHTP)₂@PPy hybrids interfacial microstructure with a unique superiority regarding EMW absorption compared with single components of PPy and Cu₃(HHTP)₂. Interestingly, the interfacial microstructure of Cu₃(HHTP)₂@PPy hybrids can be tuned by adjusting the composition of the PPy and Cu₃(HHTP)₂, resulting in the improvement of impedance matching, conductive loss, and enhancement of interfacial polarization relaxation, endowing the optimization of the EM wave absorption properties of the Cu₃(HHTP)₂@PPy. The broad effective absorption bandwidth covers a range as broad as 6.68 GHz (11.00–17.68 GHz), which is higher than most reported metal-organic frameworks (MOFs) and conductive polymer-based EM absorbing materials. Herein, new insight for developing highly efficient EMW absorption materials through hybridized interfacial microstructure engineering is provided.